Well-ordered two-dimensional (2D) hexagonal periodic mesoporous organosilicas (PMOs) with a high content of disulfide groups have been prepared by a simple metal-ions-assisted amphiphilic surfactant templating process under a strong acidic condition. Long-chain organic bridge silane, bis(triethoxysilylpropyl)disulfide (BTSPDS) was used as a precursor which can be co-condensed with tetraethoxysilane (TEOS) to assemble with the triblock copolymer Pluronic P123 template and to construct the mesostructured organica??inorganic frameworks. The content of disulfide functional groups is up to 20 (BTSPDS molar content in the initial silane mixture) incorporated into the framework. The obtained ordered mesoporous DS-PMO materials have relatively high BET surface area (580 m2/g), large uniform pore size (up to 6.3 nm) and thick pore walls (thickness up to 7.1 nm), because of the long-chain disulfide bridges. The metal ions such as Zn2+ formed the four-coordination complex with two sulfides of BTSPDS and ethylene oxide moieties of P123 template, which could enhance the interaction between the a??softa?? long disulfide groups and P123 template, thus improving the mesostructural regularity correspondingly. The disulfide-bridged PMO materials exhibit excellent hydrothermal stability in boiling water for 5 days, probably due to the thick pore walls. SEM images show that after the hydrothermal treatment, the morphology of the ordered disulfide-bridged PMO materials is retained, as that of the wheat-like SBA-15. Excellent adsorption efficiency (716 mg/g) for Hg2+ ions is observed, suggesting a potential application in removal of heavy metal ions in wastewater.